Fogged,direct-positive silver halide emulsion layer containing a cyanine dye and a compound containing a metal of group viii of the periodic table

ABSTRACT

A DIRECT REVERSAL SILVER HALIDE PHOTOGRAPHIC MATERIAL SUITABLE FOR USE IN A COPYING PROCESS ULITIZING A MERCURY OR FLUORENSANT LAMP IS PROVIDED BY INCLUDING A COMPOUND OF A METAL OF GROUP VIII OF THE PERIODIC TABLE AND A SPECIFIC CYANINE DYE IN A SILVER HALIDE EMULSION LAYER. THE FOG NUCLEI FORMED IN THE SILVER HALIDE EMULSION LAYER BEFOREHAND HAVE RESISTANCE TO INDOOR ILUMINATION, AND THE RESULTANT PHOTOGRAPHIC MATERIAL CAN BE HANDLED UNDER INDOOR ILLUMINATION WITHOUT CAUSING THE BREAKAGE OF THE FOG NUCLEI, AND GIVE IMAGES OF GOOD CONTRAST.

UnitedStates Patent US. Cl. 96-401 20 Claims ABSTRACT OF THE DISCLOSUREA direct reversal silver halide photographic material suitable for usein a copying process utilizing a mercury or fluorescent lamp is providedby including a compound of a metal of Group VIII of the Periodic Tableand a specific cyanine dye in a silver halide emulsion layer. The fognuclei formed in the silver halide emulsion layer beforehand haveresistance to indoor illumination, and the resultant photographicmaterial can be handled under indoor illumination without causing thebreakage of the fog nuclei, and gives images of good contrast.

Direct reversal silver halide photographic light-sensitive material Thisinvention relates to a direct reversal silver halide light-sensitivematerial and, more particularly, to a direct reversal silver halidephotographic light-sensitive material (hereinafter referred to merely aslight-sensitive material) suitable for a copying method wherein amercury lamp or a fluorescent lamp for copying is utilized.

As has heretofore been publicly known, in light-sensitive materials ofthis kind silver halide contained in the emulsion layer thereof isprovided with fog nuclei by exposure to light or by a chemical process,and when copying on this light-sensitive material is conducted, positiveimages can be formed by one imagewise exposure (i.e., to expose theemulsion layer imagewise to light) and one development processing.

In the above described light-sensitive material, positive images candirectly be obtained, while in the general lightsensitive materialswherein silver halide is not provided with the fog nuclei, negativeimages are formed by one imagewise exposure and development processing.Therefore, the light-sensitive materials of this kind are called directreversal photographic light-sensitive materials.

The light-sensitive material of this kind is often used as anintermediate original when many copies are prepared from blue copiessuch as a copy of diazo light-sensitive material or a blueprint. Imagesformed on the blue copies are, in the optical copying method, pretty lowin contrast. It is not preferable to use the blue copies as originalsfor copying as such'since only copies of images low in contrast can beobtained. Therefore, the blue copies are once copied to a speciallight-sensitive material (i.e., special in its constitution andexpensive too) to form images comon cheaper light-sensitive materialsusing the resulting in- 3,782,957 Patented Jan. 1, 1974 termediate imageas an intermediate original. In the copying of this type, a mercury lampor a fluorescent lamp which greatly emit light of long wavelength aswell as light of short wavelength (the light of short wavelength beingout off, for example, by using a yellow filter in order to increase thecontrast at printing) is used as a light source. Since, the color of theimages on an original is blue, which is comparatively high in lighttransmission, if light of short Wavelength strong in penetrating poweris used as a light source for exposure, the emitted light transmits theimage portions on the original to such an extent that contrast betweenthe image portions and the non-image portions is low, and hence onlyimages low in contrast can be formed in the copy obtained. Accordingly,among the light emitted fro-m a mercury lamp or a fluorescent lamp forcopying, that of comparatively long Wavelength, mainly 5460 A. and 5770A., which transmits through a yellow filter is used for the abovedescribed copying.

It has heretofore been known that in light-sensitive material formed ofa silver halide emulsion which contains a compound of a Group VIII metalin the Periodic Table, such as a rhodium salt, high in inner sensitivityand previously provided with fog nuclei, the sensitizing dyes such ascyanine dyes can be added thereto to color-sensitize, whereby thesensitivity to the light of long wavelength is raised. However, thepublicly known sensitizing dyes are not satisfactory to solve the abovementioned subject because, while they raise the sensitivity to light oflong wavelength, in many cases, they also raise the sensitivity to lightof short Wavelength at the same time. In addition, no special treatmenthas been conducted as to the peak of the spectral sensitivity in thecase of such light-sensitive materials.

On the other hand, from the standpoint of the ease of the copyingprocedure, a light-sensitive material is preferred that can be dealtwith in a bright place.

As is obvious from the reasons described above, it is preferable thatthe light-sensitive material exposed to a mercury lamp or a fluorescentlamp for copying should be high in the sensitivity to the bright linesof 5461 A. and 5770 A. in the long wavelength (both being the wavelengths at which the spectral distribution the bright lines of mercuryis maximum) among the light (i.e., the bright line of mercury) emittedfrom these light sources for exposure, and low in sensitivity to lightemitted from a fluorescent lamp used for lighting the room wherein thelight-sensitive material is dealt with, mainly to the bright lines of3660 A., 4047 A., and 4358 A. (these being the wavelengths at which thespectral distribution of the light emitted from a fluorescent lamp forroom-lighting is maximum).

Heretofore, in the case of copying a blue-image original, a copyingapparatus equipped with a mercury lamp as a light source has been used,cutting the light of wavelengths shorter than about 5000 A. by a yellowfilter. However, in such procedure, the light-sensitive material cannotbe protected from a room-lighting lamp.

The object of the invention is to provide a direct reversal silverhalide photographic light-sensitive material which is high insensitivity to light of mainly 5461 A. and 5770 A. in the longwavelength, both being wavelengths at which the spectral distribution ofbright lines of mercury emitted from a mercury lamp is maximum, andwherein the fog nuclei have resistance to breakage even when handledunder a room-lighting fluorescent lamp, i.e.,

low in sensitivity to light of wavelengths 3660 A., 4047 A. and 4358 A.among the wavelengths at which the spectral distribution of the brightlines of mercury emitted from the above described fluorescent lamp ismaximum. According to the invention, the above object can be achieved bya direct reversal silver halide photographic material wherein a silverhalide emulsion layer contains a compound of a metal of Group VIII ofthe periodic table and a dye represented by the following formulawherein L L and L, each represents a methine group, R and R eachrepresents an alkyl group or substituted alkyl group usually used forcyanine dyes, R and R each represents alkyl, aralkyl or allyl group, Xrepresents an anion, n represents an integer of 1 or 2, Z represents agoup of atoms necessary to complete a benzene or naphthalene ring, and Zrepresents a group of non metallic atoms necessary to complete anoxazole ring, and R and L and R and L respectively may be connected witheach other through an alkylene chain.

The invention will be described in detail below.

The silver halide emulsion employed in the invention is prepared bypreviously fogging a silver halide emulsion prepared in a usual mannerby a exposure to light or by chemical process using, for example,compound such as aldehydes, hydrazines, stannous chloride, silver ion,thiourea dioxide, amineborane compounds, etc. either independently or incombination. As the silver halide to be contained in the emulsion, anyof silver chloride, silver chloroiodide, silver chlorobromide, silverbromide, silver bromoiodide and silver chlorobromoiodide will do. Thegrain size thereof within the range employed in the usual silver halideemulsion is satisfactory, but a mean grain size smaller than 0.6 micronis particularly effective in the invention. The silver halide grains maybe regular or irregular grains, but regular grains bring aboutespecially good results. A monodispersed emulsion is more effective, butnon-monodispersed emulsion is also satisfactory.

These silver halied emulsions have incorporated therein with thecompound (metal salt) containing a Group VIII metal of the periodictable, such as rhodium, ruthenium, iridium, osmium, etc. The colorsensitization rate with sensitizing dyes can be remarkably raised byincorporating these metal salts. In order to raise the sensitivityfurther, salts of trivalent or tetravalent metals such as an antimony,bismuth, arsenic, etc. may be incorporated therein. In addition, thesilver halide may be subjected to chemical sensitization such asreduction sensitization, gold sensitization, sulphur sensitization, etc.Furthermore, in order to prevent the forming of negative images inexcess by exposed region, desensitizing agents such as pinakryptolyellow, pinakryptol green, phenosafranine, etc. may be incorporated.

The silver halide emulsion thus prepared which has previously beenprovided with fog nuclei can further have incorporated, as is known,developing agents such as hydroquinones, 3-pyrazolidones, etc. Inaddition, usual additives such as a coating assistant, a hardener, etc.or a color coupler may also be used in combination.

The dyes which are most characteristic of the invention are compoundshaving the foregoing general formula. The groups in the formula areexplained as follows. L L and L each represents a methine group whichmay be substituted with an alkyl or aryl group. Examples of the methinegroup are -CI-I=, C(CH C(C H and -C(C H Examples of alkyl groupsrepresented by R or R are methyl, ethyl, propyl, isopropyl, butyl andhexyl group. Examples of the substituted alkyl groups represented by Ror R are Z-hydroxyethyl, 3-hydroxypropyl, 2-methoxyethyl,3-carboxypropyl, 2-(2-carboxyethoxy)- ethyl, 2-sulfoethyl,3-sulfopropyl, 3-sulfobutyl, 4-sulfobutyl, 2-hydroxy-3-sulfopropyl,2-(3-sulfopropoxy)ethyl, 2-acetoxy-3-sulfopropyl, 3methoxy-2-(3-sulfopropoxy)- propyl, 2-{2-(3-sulfopropoxy)ethoxy}ethyl, 2hydroxy- 3 (3'-sulfopropoxy)propyl, benzyl, phenylethyl, p-sulfobenzyl,p-carboxybenzyl, p-sulfophenylethyl, and an allyl group. Examples of thealkyl groups represented by R or R are methyl, ethyl, propyl, isopropyl,butyl, etc. EX- amples of the aralkyl groups represented by R or R arebenzyl and phenylethyl group. Examples of the anion represented by X arechlorine, bromine, iodine or the residues of thiocyanate, sulfonate,perchlorate, p-toluenesulfonate, methylsulfonate and ethylsulfate. Thebenzene ring completed with Z may have substituents. Examples of theoxazole ring completed with Z, are residues of 4- methyloxazole,S-methyloxazole, 4-phenyloxazole, 4,5-diphenyloxazole,4,5-dimethyloxazole, 4-ethyloxazole, t phenyloxazole, benzoxazole,4-methylbenzoxazole, 5-meth ylbenzoxazole, 6 methylbenzoxazole, 7methylbenzoxazole, S-chlorobenzoxazole, 6-chlorobenzoxazole, 5,6dimethylbenzoxazole, 4,6 dimethylbenzoxazole, S-ethoxybenzoxazole,S-hydroxybenzoxazole, 6 hydroxybenzoxazole, alpha-naphthoxazole,beta-naphthoxazole, beta, betanaphthoxazole, etc.

When at least one of the dyes represented by the above described generalformula is added to a light-sensitive material containing the compoundsof the Group VIII metal of the periodic table, and having beenpreviously provided with fog nuclei, the sensitivity thereof to light oflong wavelength, mainly to light of 5461 A. and/or 5770 A. inwavelength, is remarkably increased and, in addition, the sensitivity tolight of short wavelength, mainly to light of 3660 A., 4047 A. and 4358A. in wavelength, is effectively reduced. Accordingly, a direct reversalsilver halide photographic light-sensitive material whose fog nucleihave resistance to breakage even when handled under a light source of aroom-lighting fluorescent lamp can be obtained.

Examples of the dyes of the foregoing general formula which bring aboutespecially good results in the invention are as follows.

Dye 1 Ha CH3 CH=CHCH= OH;

I CH3 C2Hs Br- Dye 2 HaC CHa C rncon.

CH=CH-CH= CH;

N i 41H CzHg I Dye 3 H30 CH:

CH=CHCH= I CH; C3115 Bl I Dye 14 bye 13 Dye 16 1 Dye 19 Dye'20 CH; C

CHI-- 0 H=CHa These dyes used for the invention can readily besynthesized by'reference to thedescriptionin The Cyanine Dyes and theRelated Compounds written by M.

Hamer, published by Interscience Publishers Co. in 1964, at pages62-199.

The dyes used in the invention are conveniently dissolved in a solventsuch as water, methanol, ethanol, methylCellosolve, etc., and added toan emulsion as a solution. The effective amount of the dyes to be addedto silver halide emulsion is in the range of from 1 mg. to 100 mg.,especially, from 1 mg. to 50 mg. per 1 kilogram of the emulsion.

The dyes are easily added to an emulsion immediately before coating, butthey may also be added during the ripening after rinsing, or at theformation of precipitates before that.

An example of the embodiment of the copying method using thelight-sensitive material in the invention described above is explainedas follows.

First, the light-sensitive material is imagewise exposed. The imagewiseexposure is usually carried out by superposing the light-sensitivematerial on the original in such a way that the light-sensitive layer ofthe former is closely in contact with the latter, then irradiating thesuperposed assembly with light from the side of the original or thelight-sensitive material. The former is referred to as transmissionprinting, and the latter as reflective printing. After the exposure, thelight-sensitive material is developed and, if necessary, fixed, washedand dried. The resulting copy itself may be used as a photograph, or maybe used, as is described above, as an intermediate original for copyingto a diazo light-sensitive material.

The light-sensitive material of the invention shows far more superiorcharacteristics to that of the conventional light-sensitive material ofthis kind, especially when copying is conducted using an original of lowcontrast (not being limited to a blue original) and a mercury lamp whichemits light of long wavelength as a light source. In addition, since thecopying art is utilized in every field, the invention is extremelyuseful from the industrial standpoint.

The present invention will be illustrated in detail with the followingexamples.

EXAMPLE 1 An aqueous solution of sodium carbonate was added to 1 kg. ofsilver chlorobromoiodide emulsion (containing 33 g. of silver halide,which consisted of 2 mol percent of silver bromide, 2 mol percent ofsilver iodide and 96 mol percent of silver chloride) containing mg. ofammonium rhodium chloride [(NH RhCl at the time of forming theprecipitates to adjust the pH to 8.5. Thereafter, 10 cc. of formalin (1%formaldehyde aqueous solution) was added thereto, and the mixture heatedto 40 C. for 80 minutes to form fog nuclei. Then the pH was adjusted to6.0 with citric acid and, thereafter, 10 mg. of pinakryptol yellow and 4mg. of the aforesaid dye 6 were added and coated on a photographic paperso that the amount of silver halide coated was 1.6 g; per square meterof the paper. The peak of the light-sensitive material in the sensitizedwavelength region was at a wavelength of about 545 m The light-sensitivematerial obtained in this example was exposed imagewise using anoriginal of blue diazo light-sensitive material with the use of diazocopying apparatus containing a fluorescent lamp as a light source in aroom wherein a fluorescent lamp for general lighting was lit, theilluminance in the room being 50 lux. At the time of exposure, a yellowfilter for cutting light of wavelengths shorter than 500 m was used inorder to increase contrast between the images and the background. Theprocedures of taking out the light-sensitive material from a sealedwrapper, exposing, developing and stabilizing required 40 seconds.However, there was observed no diiference in photographic propertycompared with that wherein these procedures were conducted in a darkroom. That is, it was possible to handle the lightsensitive material ina bright room under a fluorescent lamp quite safely. For comparison, thelight-sensitive ma- O\ am was used instead of the above describedsensitizing dye 6 and coated in the same manner was processed in thesame way. But in this case, when the material was processed in a brightroom the image density greatly decreased compared with when processed ina dark room. In addition, since the peak in the sensitizing wavelengthregion is at about 510 III/1., the printing sensitivity decreasedcompared with that of the dye of this invention, and hence the dye wasrequired in an amount about 3 times as much as that of the dye of thisinvention in order to obtain the same printing sensitivity.

EXAMPLE 2 An aqueous solution of sodium carbonate was added to 1 kg. ofsilver bromoiodide emulsion (containing 43 g. of silver halideconsisting of 2 mol percent of silver iodide and 98 mol percent ofsilver bromide) containing 40 mg. of potassium ruthenium chloride [KRuCl at the time of forming the precipitates to adjust the pH to 9.0.Thereafter, 3 cc. of 1% aqueous solution of hydrazine hydrochloride and1 cc. of 0.01% aqueous solution of potassium chloroaurate were addedthereto, and it was heated to 45 C. for minutes to form fog nuclei.Then, the pH was adjusted to 5.5 with citric acid and, thereafter, 5 mg.of pinakryptol green and 5 mg. of the aforesaid dye 2 were added and theresultant solution coated on a polyethylene terephthalate photographicfilm so that the amount of silver halide coated was 3 g. per squaremeter of the film.

The peak of the light-sensitive material in the sensitized wavelengthregion was at the wavelength of about 540 m The light-sensitive materialobtained in this example was exposed imagewise using a blue diazooriginal with the use of a diazo copying apparatus containing a mercurylamp in a room wherein a fluorescent lamp for roomlighting was lit, theilluminance in the room being 50 lux. The procedures of taking out thelight-sensitive material from a sealed wrapper, exposing and developingit (a rapid processing apparatus which automatically conducts thedevelopment, fixing, washing and drying was employed) required seconds.During this period, the light-sensitive material was exposed to theroom-lighting lamp for 40 seconds. However, there was observed nodifference in photographic property compared with that wherein theseprocedures were conducted in a dark room. That is, it was possible tohandle the light-sensitive material quite safely in a bright room undera fluorescent lamp. For comparison, the light-sensitive material wherein13 mg. of the dye represented by the following formula:

was used instead of the above described sensitizing dye and coated inthe same manner was processed in the same way. But in this case, whenthe material was processed in a bright room, the image density greatlydecreased compared with when processed in a dark room.

In addition, since the peak in the sensitized wavelength region is atabout 510 my, the printing sensitivity decreases compared with that ofthe dye of the invention, and hence the dye was required in an amountabout 2.6 times as much as that of the dye of the invention in order toobtain the same printing sensitivity.

9 EXAMPLES An aqueous solution of sodium carbonate was added to 1 kg.offsilver chlorobromoiodide"emulsion(containing g. of silver halideconsisting erg mol percent of silver iodide, 20 mol pergent of silverbromide and 78 mol percent of silver chloride) containing 1Q mg. ofpotassium iridiumchloride.i[K IrCl at the time of forming theprecipitates to adjust the pH to 8.5. Thereafter, 10 cc. of formalin(1%{ormaldehyde aqueous solution) was added thereto, and it was heatedto C. for 85 minutes to form fog nuclei. Then the pH was adjusted to 5.5with citric acid and, thereafter, 1Q mg. of pinakryptol yellow and 3 mg.of the aforesaid sensitizing dye 18 were added and coated on aphotographic paper so that the amount of silver halidecoatedfwas 1.9 g.per lgsquare meter of the paper. The peak of the resultinglightesen'sitive material in the sensitized wavelength region was atabout 552 mu.

The light-sensitive material obtained in, this example was exposedimagewise using a blue diazo original with the use of a diazo copyingapparatus containing a fluorescent lamp therein in a room wherein afluorescent lamp for room-lighting was'lit," the 'illuminance in theroom being lug. procedures of taking out the lightsensitivematerial'from a sealed wrapper, exposing, developing and stabilizing itrequired 40 seconds. However, there was observed no difference inphotographic property compared with that wherein these procedures wereconducted in a dark room. That is,it was possible to handle thelight-sensitive material quite safety in a bright room underafluores'cent lamp.

For comparison, the light-sensitive material wherein 13 mg. ,of. the dyein the Example 1 forcomparison was used and coated in the same way wasprocessed in the same manner. But 1 in" this case, when the material wasprocessed in a bright room the image density greatly decreased comparedwith when processed in a dark room.

In addition, since the peak in the sensitize'd'wavelength region is atabout 510mb, the printing-sensitivity decreased compared with that ofthedye of this invention, and hence the dye was required in. an amountabout 4 times as muchasthat of the dye of this invention in order toobtainthesanie printing sensitivity.

What is claimedisf 1. A direct reversal silver halide; photographiclightsensitive material used in the copying method in which the brightlines [of mercury, mainly'of-5460 A. and 5770 A. in wavelength, areutilized as a light source, wherein a silver halide emulsion layer,whose silver halide grains are uniformly fogged, provided onthelight-sensitive material has incorporated therein a compound containinga metal of groupVIII of the periodic table, said compound increasing thecolor. sensitization of the emulsion by a sensitizing dye, and a dyerepresented by the following formula wherein-L L and each represents-amethine group; R and R each represents an alkyl group or a sus'btitutedalkyl group wherein said alkyl group or saidsubstituted alkyl group areof the type usually employed as a N-sub stituent inwcyaninedyes; R and Reach represents an alkyl, aralkyl or allylgroup; X represents an anion;n represents aninteger of"1*"or' 2; Z represents a group of atomsnecessary co, complete a benzene or naphthalene ring; and Z represents agroup of non-metallic atoms necessary to complete an oxazole ring;wherein R and R 10 and R and L respectively, may be connected with eachother through an alkylene chain.

2. Thephotographic material of claim 1, wherein the amount of said dyeis 1 to mg. per kilogram of said emulsion layer.

3. The photographic material of claim 1, wherein the amount of said dyeis 1 to 50 mg. per kilogram of said emulsion layer.

4. The photographic material of claim 1, wherein said emulsion layerfurther contains a salt of a trivalent or tetravalent metal to furtherincrease the color sensitization of the emulsion by said sensitizingdye.

5. The photographic material of claim 1, wherein said emulsion layerfurther contains a desensitizer.

6. The photographic material of claim 1, wherein said emulsion layer ischemically sensitized.

7. The photographic material of claim 1 wherein the mean grain size ofsaid silver halide grains is less than 0.6 micron.

8. The photographic material of claim 1 wherein said metal is rhodium,ruthenium, iridium or osmium.

9. The photographic material of claim 4 wherein said trivalent ortetravalent metal is antimony, bismuth or arsenic.

10. The photographic material of claim 1 wherein said methine group issubstituted with an alkyl or an aryl group. g

11. The photographic material of claim 10 wherein said substituent ismethyl, ethyl or phenyl.

12. The photographic material of claim 1 wherein the alkyl of said R andR has from 1 to 6 carbon atoms.

13. The photographic material of claim 12 wherein the substituent ofsaid substituted alkyl group is hydroxy, alkoxy, carboxy, sulfo,acetoxy, aryl or vinyl.

14. The photographic material of claim 13 wherein said substituted alkylgroup is selected from the group consisting of Z-hydroxyethyl,3-hydroxypropyl, 2-methoxyethyl, 3-carboxypropyl,2-(2-carboxyethoxy)ethyl, 2-sulfoethyl, 3-sulfopropyl, 3-sulfobutyl,4-sulfobutyl, 2-hydroxy-3-sulfopropyl, 2-(3-sulfopropoxy)ethyl,-2-acetoxy- 3sulfopropyl, 3-methoxy-2-(3-sulfopropoxy)propyl, 2 {2-(3-sulfopropoxy)ethoxy}ethyl, 2-hydroxy 3 (3 sulfopropoxy)propyl,benzyl, phenylethyl, p-sulfobenzyl, p-carboxylbenzyl,p-sulfophenylethyl, and allyl groups.

15. The photographic material of claim 1 wherein the alkyl of said R andR has from 1 to 4 carbon atoms.

16. The photographic material of claim 15 wherein said 1aralkyl group ofsaid R and R is benzyl or phenylet y 17. The photographic material ofclaim 1 wherein said anion is chlorine, bromine, iodine, 'thiocyanate,sulfonate, perchlorate, p-toluenesulfonate, methylsulfonate orethylsulfate.

18. The photographic material of claim 1 wherein said oxazole ring isselected from the group consisting of 4-methyloxazole, S-methyloxazole,4-phenyloxazole, 4,5- diphenyloxazole, 4,5-dimethyloxazole,4-ethyloxazole, tphenyloxazole, benzoxazole, 4-methylbenzoxazole, 5-methylbenzoxazo'le, 6-methylbenzoxazole, 7-methylbenzoxazole,S-chlorobenzoxazole, 6-chlorobenzoxazole, 5,6- dimethylbenzoxazole,4,6-dimethylbenzoxazole, S-ethoxybenzoxazole, S-hydroxybenzoxazole,fi-hydrox ybenzoxazole, alpha-naphthoxazole, beta-naphthoxazole andbetanaphthoxazole.

19. Thephotographic material of claim 1 wherein said dye is selectedfrom the group consisting of 13 14 mo CH, 20. The photographic materialof claim 1 wherein said compound of said metal is an ammonium metalchloride /0 or a potassium metal chloride.

}"CH=CH*CH= C104 5 References Cited 13 UNITED STATES PATENTS I 12,717,833 9/1955 Wark 96--108 d CHCHCOOH 1 3,531,288 9/1970 Jones 96-408m 3,567,456 3/1971 Riester et a1 96-134X H3O CH; 10

\ o NORMAN G. TORCHIN, Primary Examiner W. H. LOUIE, JR., AssistantExaminer /-GH=CH-CH= I 15 US. Cl. X.R. N f 96-107, 108, 125, 137

